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Volumn 111, Issue 21, 1999, Pages 9673-9677

Glass-like behavior in supercritical fluids: The effect of critical slowing down on solute dynamics

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[No Author keywords available]

Indexed keywords


EID: 0000285699     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.480299     Document Type: Article
Times cited : (23)

References (56)
  • 7
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    • edited by P. v. R. Schleyer, N. L. Allinger, T. Clark, J. Gasteiger, P. A. Kollman, H. F. Schaefer III, and P. R. Schreiner Wiley, Chichester
    • S. C. Tucker, in The Encyclopedia of Computational Chemistry, edited by P. v. R. Schleyer, N. L. Allinger, T. Clark, J. Gasteiger, P. A. Kollman, H. F. Schaefer III, and P. R. Schreiner (Wiley, Chichester, 1998), p. 2826.
    • (1998) The Encyclopedia of Computational Chemistry , pp. 2826
    • Tucker, S.C.1
  • 14
    • 85034152217 scopus 로고    scopus 로고
    • note
    • Relative to an ideal gas.
  • 21
    • 0003796670 scopus 로고
    • edited by R. Balian, R. Maynard, and G. Toulouse World Scientific, Singapore
    • P. W. Andersen, in Ill-Condensed Matter, edited by R. Balian, R. Maynard, and G. Toulouse (World Scientific, Singapore, 1979).
    • (1979) Ill-Condensed Matter
    • Andersen, P.W.1
  • 26
    • 85034120529 scopus 로고
    • ACS Symposium Series 488, edited by F. V. Bright and M. E. P. McNally ACS, Washington, DC
    • T. A. Betts, J. Zagrobelny, and F. V. Bright, in Supercritical Fluids, ACS Symposium Series 488, edited by F. V. Bright and M. E. P. McNally (ACS, Washington, DC, 1992).
    • (1992) Supercritical Fluids
    • Betts, T.A.1    Zagrobelny, J.2    Bright, F.V.3
  • 27
    • 85034137406 scopus 로고    scopus 로고
    • note
    • In a similar vein, Procaccia and Gitterman (Refs. 49, 50) suggested that critical slowing down would slow reaction rates, but their analysis was later demonstrated to be in error (Refs. 51 and 52).
  • 28
    • 85034150286 scopus 로고    scopus 로고
    • note
    • -ν) is ν=0.63 and 1.0 in three and two dimensions, respectively. This expected similarity between 2D and 3D supercritical behavior has already been validated by two recent results. First, preliminary simulations of a 3D supercritical Lennard-Jones fluid by H. L. Martinez, S. G. Srinivasan, and S. C. Tucker show qualitatively similar local density behavior as was observed in 2D supercritical Lennard-Jones fluids (see Refs. 22, 38, and 53). Second, we have recently demonstrated (Ref. 39) that the 2D system studied herein reproduces the density-dependence observed experimentally for vibrational relaxation lifetimes in 3D supercritical fluids.
  • 30
    • 85034125305 scopus 로고    scopus 로고
    • note
    • The mass of each atom comprising the diatomic is the same as the solvent mass.
  • 34
    • 85034132018 scopus 로고    scopus 로고
    • note
    • LJ, and both neighbor listing and periodic boundary conditions were employed. At each state point, the system was equilibrated for 80 000 time steps, during which velocity rescaling was performed every 31 times steps. Data were subsequently collected over 1000 blocks of 4000 time steps each, with 200 time-step velocity-rescaled equilibrations occurring between blocks.
  • 35
    • 85034128300 scopus 로고    scopus 로고
    • note
    • LJ here.
  • 36
    • 85034133125 scopus 로고    scopus 로고
    • note
    • b solvent forces on sites a and b of the diatomic, respectively, and Ω the diatomic's orientation vector.
  • 37
    • 85034154421 scopus 로고    scopus 로고
    • note
    • / ≳ 3 are not significantly influenced by the detailed packing geometry of the solvent. See Ref. 22 for an in-depth discussion of this issue.
  • 42
    • 0001585297 scopus 로고    scopus 로고
    • It is still unknown, however, why theory and experiment often fail to predict the same magnitude anomalies. See, for example, J. E. Adams, J. Phys. Chem. B 102, 7455 (1998).
    • (1998) J. Phys. Chem. B , vol.102 , pp. 7455
    • Adams, J.E.1
  • 43
    • 85034151055 scopus 로고    scopus 로고
    • note
    • Although not obvious from Fig. 2, approximately 1 solute molecule in 1000 has no solvent neighbors in its local region.
  • 47
    • 85034151352 scopus 로고    scopus 로고
    • note
    • / are permitted in the integral.
  • 54
    • 85034123851 scopus 로고    scopus 로고
    • note
    • LJ, with a correlation of R = 0.989.
  • 56
    • 85034152375 scopus 로고    scopus 로고
    • note
    • We generated this curve using the Gaussian fit in Fig. 4 and Ref. 54.


* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.